An arene-tethered silylene ligand enabling reversible dinitrogen binding to iron and catalytic silylation.

An arene-tethered silylene ligand, L (L = PhC(tBuN)2SiCH2C(tBu)NAr, Ar = 2,6-iPr2C6H3), allowed the synthesis of three-coordinate Fe(ii) silylamido and piano-stool Fe(0) dinitrogen complexes LFe[N(SiMe3)2]2 (3) and LFe-N2 (4), which not only exhibit interesting bonding but also enabled the catalytic silylation of N2 to yield N(SiMe3)3 under 1 atm of N2 at room temperature with high TONs.